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Polymer–MOF Hybrid Composites with High Porosity and Stability through Surface-Selective Ligand Exchange

Cite this: Chem. Mater. 2018, 30, 23, 8639–8649
Publication Date (Web):November 17, 2018
https://doi.org/10.1021/acs.chemmater.8b03881
Copyright © 2018 American Chemical Society

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    Abstract

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    Hybrid materials containing organic polymers and metal–organic frameworks (MOFs) have attracted attention for their potential to harness both diverse functionality and high processability, but their fabrication is challenged by incompatibilities of the parent components. The poor solubility of MOFs hinders uniform dispersion throughout a polymer matrix and may cause aggregation that is not only detrimental to the permeability of substrates, but also limits the structural integrity of the polymer. Meanwhile, polymer chains can block or penetrate the porous structures and compromise MOF functionality by reducing surface area and pore size. We report a versatile method of covalent hybridization through post-synthetic ligand exchange to form a cross-linked polymer–MOF composite. The resulting network structure allows for the formation of robust, monolithic composites with variable MOF loadings that may exceed 80% wherein ligand exchange is limited to surface sites so as to fully preserve MOF surface area and porosity. The synthesis can be performed from a diverse set of inexpensive starting materials, encouraging the design of new functional materials across a wide range of applications.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.chemmater.8b03881.

    • Video of composite formation (MPG)

    • PXRD diffractograms of MOF-5, PAA, MOF-5/PAA, and MOF-5/PI; PXRD diffractograms of ZIF-8 and ZIF-8/MOF-5 composites; PXRD diffractograms of UiO-66; 1H NMR spectrum of PAA; 1H NMR spectrum of MEPA; 1H NMR spectrum of PVBA; GPC traces of PAA-high, PAA-low, and MEPA; polymer molecular weight data; SEM images of free polymer-coated MOF-5; FT-IR spectra of PAA and PI; FT-IR spectra of MOF-5/PAA and MOF-5/PI; TGA curves of microcrystalline MOF-5, PAA, and microcrystalline MOF-5/PAA; TGA curves of nanocrystalline MOF-5, PAA, and nanocrystalline MOF-5/PAA; TGA curves of ZIF-8, PAA, and ZIF-8/PAA; DSC curves of PAA, microcrystalline MOF-5/PAA, nanocrystalline MOF-5/PAA, and ZIF-8/PAA; N2 adsorption–desorption isotherms of ZIF-8 and ZIF-8/PAA; and N2 adsorption–desorption isotherms of nanocrystalline MOF-5 and nanocrystalline MOF-5/PAA (PDF)

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